Injection nozzle



D. H. BARBOUR ETAL 2,804,339

INJECTION NOZZLE Aug. 27, 1957 Filed March 30, 1955 INVENTORS DANIEL H.BARBOUR ALBERT HOFFMAN,JR Ma/1.2M

ATTORNEY 2,34,339 Patented Aug. 27, 1957 INJECTION NOZZLE Daniel H. Barbour and Albert Hoifman, Jr., Niagara Falls, N. Y., assignors to Union Carbide Corporation, a corporation of New York Application March 30, 1955, Serial N 0. 498,073

2 Claims. (Cl. 209-107) This invention relates to a nozzle for 'efiecting the introduction of fluids into a reactive medium, and more particularly to a nozzle for efiecting the injection of a stream of molten material at substantially high temperature and at substantially high velocity, into a reactive medium.

The metallurgical industry has long sought a practicable means of producing refractory metals, particularly those high melting point refractory metals of groups IV, V and VI of the periodic table, many of which are reducible only with difficulty. Ordinary metallurgical procedures are not applicable to most of these metals and special techniques have been evolved for procuring the elements in metallic form. The currently proposed processes are generally based upon reduction of the refractory metal halide by one of the metals of the alkali or alkaline earth metal groups, since, the latter havea greater afiinity for halogens than is generally true of the refractory metals. These reduction processes are usually highly exothermic and therefore rather difficult to control.

The increasing industrial demand for these metals has been responsible for increased efforts to find a commercially feasible method for their production. One of the paramount problems faced is that of introducing the reactants to each other.

Many major difiiculties are encountered in feeding fluids into reactive media. This is particularly true when such reactions are conducted at elevated temperatures, when solid products are formed as a result of the reaction, where safety is a consideration, or where the reaction is exothermic. Agitation is of course required in order to assure proper contact between the. reactants, but agitation also presents serious problems. Continuous mixing of the reactants is necessary since segregation of one or the other results in large irregularities in the rate of heat evolution, and should large quantities suddenly come into contact with each other, the very large amount of heat suddenly evolved might severely damage the reaction chamber, either by virtue of the great in crease in temperature or pressure that may ensue.

Another difliculty which may arise is due to the reaction occurring between the vapors of the reactants, the

solid products of the reaction then being deposited on the upper walls of the reactor and more particularly around.

any openings through which either of the reactants may be introduced into the reaction chamber. Should such openings become closed over as a result of such deposition of solid material, it becomes impossible to continue the operation unless some special devices are provided for removing such obstructions without the necessity of opening the reactor.

As an example of a reaction having the difiiculties and problems enumerated, the reduction ofrefractory metals from their halides by a molten reducing metal may be cited. Selecting as a specific example that of the reduction of chlorides of titanium to titanium metal by a molten reducing metal such as sodium metal or magnesium metal, these problems are immediately apparent.

The necessary agitation, for reasons of both contact between the reactants and safety, cannot be achieved by mechanical means since it is impractical to operate and lubricate bearings at high temperatures in the presence of corrosive materials, and a long unsupported shaft with an impeller at its extended end will not operate satisfactorily, since at high temperatures the shaft loses much of its rigidity and the impeller will not remain in its proper location Within the reaction. vessel. Attempts to use such mechanical devices to provide agitation within the reacting mass have resulted in the puncturing of the wall of the reaction vessel when the shaft became bent and whipped around within the enclosure. Also,

' deposition of solid products of the reaction dynamically unbalance therotor and add to the difliculties of its use. Further, there is a tendency for the reduced metal to form on the sides of the reaction chamber, necessitating a difiicult and costly removal.

The objects of the present invention are therefore to avoid the difficulties referred to above, to elfect the introduction of fluid at high temperature and high velocity into a reactive medium in a cohesive uninterrupted stream, to minmize vaporization of the material from the stream, to eifect self-cooling, to effect complete and ultimate mixing of the reactants, and to minimize the possibility of deposition of solid reaction products on the end of the nozzle and thus avoid interference with the fiow of the injected liquid.

The invention by means of which the objects herein are achieved comprises a special nozzle structure for injecting a reducible refractory metal halide or alkali or alkaline earth metal in the liquid state into a molten educing metal at high velocity into a reactor where reaction takes place to produce the high melting point refractory metal in elemental form. Preferably the re actant with the higher boiling point, and consequent lower vapor pressure-temperature relationship is first placed in the reactor and the other reactant injected through the nozzle.

In order to produce the desired result, the nozzle must have certain characteristics and meet certain rigid requirements. These requirements will be described herewith.

In order to reduce the possibility of vapor-phase reactions, it is essential that the stream of reactant thus injected should remain as a coherent body of liquid and should not separate into discrete droplets at any time during its passage from the nozzle to the surface of the reactant bath in the bottom of the chamber.

As is well known in the art, fluids flow through tubular containers in two distinct and characteristic manners. In one case, called viscous'flow, the velocity of the liquid is substantially uniform throughout its cross-sectional area, except immediately adjacent to the walls of the tubular container where the velocity is gradually reduced to an extremely low value at the contact surface between the fluid and the tube. In the other case, turbulence occurs within the liquid and the velocity is nowhere uniform Within the body of the liquid. It has been established that the difierence between viscous or streamline flow and turbulent flow is dependent upon the mean velocity of the liquid, the diameter of the tube, the specific gravity and the absolute viscosity of the liquid. A formula developed by Reynolds relates these factors as follows:

VDs

When these quantities are expressed in c. g. s. units and the value obtained from the calculation is less than about 2,000, in general, streamlined or viscous flow occurs.

when the value exceeds'LGQQ, turbulent flow may usually e sta h d- I s essent a 9t course that this criterion be taken into account in designing a nozzle for the instant application, since streamlindfiow is essential to product tan at a c herent strea Q jec ed liq d- Th fifln 9 the 1? must be s h as to. preven efle t 9? th in e d s e m o reactant y d position 5? nannie 9 the eac on. Preve io of accnmuii 9f 91 reast h r d a 9 e noz l is achi ved i .3 159 menus. y' e u at h the't ipe a ure'c the #0???- I a sh nd tha ft e nozzle a e kep 99 1 99 fl fiih it Of m er l th s d pos ed s g e y.

factory results have been obtained with the length to Qt?! li itl t as 10W .815 lythe preferred range is 5 to 20. T e design of the exit end of the nozzle throat is also of some importance, and this design is shown in detail in an enlarged form in Fig. 2. It is necessary that the design at the exit end of the nozzle throat be such that there is a. clean breaking away of the liquid stream from the body of the nozzle with little or no tendency to separate droplets from the stream or to accumulate liquid on the outer surface of the nozzle body. The square'cut design shown in the Fig 2 has been found to be preferable. The

reduced. However, water cooling is completely impracii a tt a ety asQ s-l T e m nut s; rear woul not ta 9. sqa amiha e the me a ic Produc as to i us ess t t it would eact w h the a kal or a k ine earth Phi wi h ssi i Fl $t l re ult t' is eces y,

t t re that th n zzle be. e ned s s t e c oled ae ial goi th o h t In a di on, since. he ,fqi tql Pr du ts en under he e t otcirhee ah, qa thg be nt rely pr v n ed it s c ary at he cohtl hrat s of henpzz e e su h t atinterf ronce of such deposits with the coherence of the liquid s ream. be en i e y el in ed h sswt Psnyh d w s a schema p e n a: tion bf'an' ,mhog i n nt t e nven i n whereby he obiectsfof the invention may be achieved.

1 dra i Figfl is a sectional side view of a nozzle aocording 9 e. i veati h; and

Fig. Zis an enlargement of the exit port shown inFig, l. Thea-nozzle of the invention comprises an elongated body prep ared from any metal possessing suitable corro: sion resistance under the operating conditions. The body has a 1 9? e ,0 and an l t nd. nd. a. sub anstr aight longitudinal bore 13 therethrough forming an inlet port14at the inlet end 10 and an exitport 15, at

th e outlet 1 2. The inlet end 10 is adapted in any su ta e mann r f r s amp Y hre d .6, o comhh sa W th fl d hpp 0 7 .1 h gushthe nozzle has a smoothly reduced taper 11 fro nithe inlet, Pa o a m nt ab ut WQ- s he eng h of, hehore from the inlet port 14, The remainder of the, bore, 18; has a substantially constant diameter,andterminages. at, the e? P r 1. n an u wa y fl ri g Por on. 940 qh ta t y inc ea n r s r qti n'a ea: The external; P9ti f the qa e RQES mo h y ro he i let i 10 towards the outlet end 12 to a relatively thin Wall thickness, ,so that the liquid fiowingthrough thenozzle keeps the tip relatively cool. The tapered outer. wjallv terminatesso as toforrn a junction 29 withtheoutwatd y,

flaring portion l jg ofthe longitudinal bore 1 3,.

cooling effect isfurtherjenhenfied, by the interior. configuration, whiclris such as to maintaina relatively, thin wall thickness throughout the nozzle. In order. to l llti fi. ny arbh sht ew h h m y he trodu ed: y. the change in diameter from the feed ipe, to, the. nozzle and with in the nozzle, the tip sectionis preparedwith a bore of uniform diameter. For satisfactory results, it is. necessary that the ratio of the length of, this cylindrical. bore section to the diameter be within, certainlimits and, in "accordance with the formula previously expressed, for. the particular liquid andinjection velocity, the dimen: sions of the nozzle boreat the tip must be such that when, inserted into the formula together with the other required quantities, a'Reynolds number'of less than 2,00Qwill be obtained. I The relationship between the diameterofthe, nozzle opening and the length of the cylindrical section is believed to be related to the time required. foil cessation of turbulent flow and the establishment. viscous flow, and it is further, believed that this may be related to the viscosity of the liquid, and, of course, the velocity of its passage through the nozzle. Obviously, the greater the velocity and ease Ofdisturbanee offlow pattern within the liquid, the longer the cylindrical por;

t of the tip must be. Although somereasonably satiswidth of the face at the thief the nozzle, however, is keptto a very small dimension in order to provide no foothold for the accumulation of solid products of the reaction.

By use of the nozzle of the invention the difiiculties and problems in producing refractory metals as heretofore set forth are satisfactorily eliminated. Using the example of the reduction of titanium tetrachloride to titanium metal by a molten reducing metaLthe reaction is carlfit d. O lt'iu a suitable chamber closed at both ends, Preferably with its longitudinal axis vertical, into the bottom of which, an ap ropriate charge. of reducing metal is placed. Extending through the upper cover of the chamberis thenozzle of the. invention through which titanium chloride is introduced, into the chamber and into the molten reducing metal. The reaction is preferably carrie'diout'in an inert atmosphere. a i The reaction is initiated by heating the reducing metal to.a temperature suthcient to liquefy it, and then introducing the liquid titanium tetrachloride at high velocityby means of the nozzle of the invention so that the liquid is injected into substantially the central portion of the body ofzriiolten metal and becomes immediately and intimately mixedftherewithand at least partially reduced, before any appreciable vaporization occurs. The nozzle of the invention permits the stream of titanium tetrachloride to be sodirected that impingement occurs within the central portion of the mass of molten reducing metal and the heat generated-by the reaction is dissipated throughout the soiid ioductsfmayfocicur atthe exit end of the. nozzle, eflect -the stlream 'off titanium tetrachloride.

agtfth e exit JildflfthQ nozzle is relatively very thin, but e d' rid theitaperi of the'external conical ,should a1 deposit. build up in that surface there lS VGIfY littleflikelihood that it will extend into "and, deflect the stream of titanium tetrachloride the nozzle. Further, in the event that such ould occur, the nozzle is preferably mounted Chieof the, riibstin'iportaneadvantages of the use of the velocity stream according. "tof the method of the lies m1its'fgre'atrsupeiiorityv over agitation by rnchanical'ineafis. When a liquidina relatively narrow Stream n e r tt elahr lrh h lsi hath. hwa tent, a f hs m i nsarohh ah i a stu n resulting nan mme ate htl t at sal hi e at. ubstant ally, t t y o e ntact between thev reactants so brought together. In effect,

anieans of, adding one reactant to another results,

nfat the, chamber, surfaces, some deposition of.

V f o this'occurring is materiallyreduce d;by fii se O ha zle fthe lenfiPnl thick ess.

in the bringing together of the reactants in such a manner and at such a rate so as to be reacted immediately upon their contact with each other. A further advantage resulting in such a means of efiecting the reaction is that the rotating motion set up within the reactant mass tends to cause formation of the reduced metal as a compact sponge suspended in the central portion of the molten fluid which greatly facilitates removal of the reactive products from the reaction vessel. Also, since very little reaction occurs outside themain mass of molten metal and metallic chlorides, the metal reduced during the reaction is protected from contamination by either the reaction vessel or vapors within the space above the reacting mass, and metal of unusual purity is obtained.

The invention has been used for injecting titanium tetrachloride, tantalum pentachloride, and sodium metal into reactors of various sizes, and has proved eminently satisfactory in operation and free of clogging difiiculties.

For example, titanium tetrachloride was injected through the nozzle at feed rates of 120 pounds per hour for the first 10%, 180 pounds per hour from 10 to 20% and 240 pounds per hour for the remainder of the run period. The reaction proceeded smoothly, and temperature distribution was uniform. The nozzle had a 0.047 inch internal diameter. At the end of the run, the nozzle was found to be clean and free of interfering deposits.

Typical nozzles that have been successfully employed for the above-stated purposes and which embody the principle of the invention are described in the following examples.

EXAMPLE I In a relatively small capacity reaction system, two sizes of nozzles were used under varying conditions with completely satisfactory performance. Table I presents the pertinent information.

In another operation on a somewhat larger scale, nozzles of the same design but having slightly different dimensions were employed with satisfactory results. The pertinent data are presented in Table II.

Table II Injection Feed Rate Bore Bore Ratio, Dia., In. Leirlgth, l./d. 1b./min. feet/sec.

max. min. max. min.

EXAMPLE III In still another operation, nozzles of the invention but of large internal diameter were used, as shown in Table III.

Table III Injection Feed Rate 1 B0re Bore Ratio, Dia., In. Leiingth, l./d. lb./min. feet/sec.

max. avg. max. avg.

EXAMPLE IV Table IV Injection Feed Rate Bore g s Ratio, Dia., in. l./d.

- lb./min. tt./min.

avg. avg.

EXAMPLE V In an operation where the molten reducing metal was injected into the reactor, a nozzle of the invention was employed. The molten metal was not filtered and some plugging occurred during the test, but aside from this, the operation was satisfactory. Details are given in Table V.

Table V Injection Feed Rate Bore Bore Ratio, Dia., In. Leilgth, l./d. 1b./min. feet/sec.

max. min. max. min.

We claim:

1. A nozzle for delivering fluids of reactive molten material and injecting them into a reactor in a viscous flow at substantially high temperatures and at substantially high velocities, comprising an elongated body constructed of rigid corrosion resistant metal capable of withstanding said high temperatures and velocities and having inlet and outlet ends, a substantially straight longitudinal bore therethrough forming an inlet port at said inlet end and an exit port at said outlet end, said inlet end being adapted to communicate with means for supplying said reactive molten fluids to said inlet port, said bore having a smoothly reduced taper from said inlet port to a point about twothirds the length of said bore from said inlet port, the remainder of said bore having a substantially constant diameter and terminating at said exit port in an outwardly flaring portion of constantly increasing cross-sectional area, the ratio of the length of said taper to the length of said constant diameter producing viscous flow in a continuous uninterrupted stream to effect self-cooling of the nozzle and complete and ultimate mixing of the reactants, and the external portion of said nozzle tapering smoothly from said inlet towards said outlet end and terminating so as to form a junction with said outwardly flarifigfiortions of said here to prevent deposition of solid p r o diicts oftlie reaction and consequent deflection of the injected stream. a

2. A iioizle for injecting reactive molten materials into a reactor in viscous flow at substantially high temperatures and at substantially high velocities, comprising anelo ng'atedlbody of rigid corrosion resistant metal capable. of withstanding isaid high temperatures and veloci'ties; and having inlet and outlet ends, a longitudinal bore therethrough fprrning an inlet port at the inlet end and w n ezitrzqrtat he qutlstend, id inlet end being adapted to be connected to a conduit for supplying said reactive molten material to said inilet port, said bore having a 15 smoothly reduced: taper from said inlet port to about two thirds ofi 'its lengthy the remainder of said bore being cylindrical: and terminatingat said exit port in an outwardly flaring portion "of constantly increasing cross sec- Qdii s us-fla qm n 'c is ed strearnto et fectselficoqling of the nozzle the outside of said body tapering smoothly fr m near said lnle t end toward th eoutlet end, and terminating in a junction with said outwardly flaring portion of said bore, the i qft c en th 9 h c i d c l p rti o e diameter ofthe nozzle opening being between 5 and 20.

References Cited in the file of thispatent 'UNLTED. STATES PATENTS 1,046,043

and complete and'ultirnate mixing of the reactants, and, 

